Insights into the electron transfer regime of permanganate activation on carbon nanomaterial reduced from carbon dioxide

Jingquan Wang; Zhizhuo Chai; Shuai Yang; Erdeng Du; Hongguang Guo

doi:10.1016/j.jhazmat.2023.132094

Insights into the electron transfer regime of permanganate activation on carbon nanomaterial reduced from carbon dioxide

J Hazard Mater. 2023 Oct 5:459:132094. doi: 10.1016/j.jhazmat.2023.132094. Epub 2023 Jul 20.

Authors

Jingquan Wang¹, Zhizhuo Chai¹, Shuai Yang¹, Erdeng Du², Hongguang Guo³

Affiliations

¹ MOE Key Laboratory of Deep Earth Science and Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China.
² School of Environmental and Safety Engineering, Changzhou University, Changzhou 213164, China.
³ MOE Key Laboratory of Deep Earth Science and Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China. Electronic address: hgguo@scu.edu.cn.

PMID: 37515988
DOI: 10.1016/j.jhazmat.2023.132094

Abstract

Simultaneously eliminating novel contaminants in the water environment while also achieving high-value utilization of CO₂ poses a significant challenge in water purification. Herein, a CO₂-reduced carbon catalyst (CRC) was synthesized via the chemical vapor deposition method for permanganate (PM) activation, fulfilling the ultra-efficient removal of bisphenol A (BPA). The primary mechanism responsible for the BPA degradation in the CRC/PM process is electron transfer. Hydroxyl groups and defect structures on CRC act as electron mediators, facilitating the transfer of electrons from contaminants to PM. On the basis of the quantitative structure-activity relationship, the elimination performance of the CRC/PM process exhibited variability in accordance with the inherent characteristics of pollutants. In addition, the yield of manganese intermediates was also observed in the CRC/PM process, which only serve as redox intermediates rather than active species attacking organics. Ascribed to nonradical mechanisms, the CRC/PM system exhibited remarkable stability and demonstrated significant resistance to the presence of background substances. Moreover, BPA degradation pathways were clarified via mass spectrometry analysis and density functional theory calculations, with intermediate products exhibiting lower toxicity. This study provided new insights into the employment of carbon catalysts derived from CO₂ for PM nonradical activation to degrade contaminants in various water matrices.

Keywords: Bisphenol A; Carbon dioxide; Electron transfer; Permanganate; Theoretical calculation.